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CSSC 201801690
CSSC 201801690
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Supporting information for this article is given via a link at the end of
the document.
feedstocks and potentially integrate with existing industries and ASTM D1655 Standard Specification for Aviation Turbine
supply chains. In addition, there has been little economic study Fuels[16], and details the requirements for petroleum distillates
centered on the technological details of the catalytic upgrading meeting a certain distillation curve and other properties deeming
steps providing the foundation for the ATJ pathway (dehydration, them “fit-for-purpose”. A standard for alternative jet fuels is
oligomerization, hydrogenation, and fractionation) and how their contained in ASTM D7566 Standard Specification for Aviation
implementation varies depending on the feedstock and alcohol Turbine Fuels Containing Synthesized Hydrocarbons [3], which
fermentation process used[10]. provides additional pathways to qualified fuels through an
In this paper, we will expand upon these data by individually added annex for each fuel. The standard is regularly
constructing process economic models for the ATJ pathway updated and new fuels may be added through an extensive and
using both an ethanol and an isobutanol intermediate. Process rigorous review process set forth by ASTM D4054 Standard
simulation and predesign cost estimation will be used to Practice for Qualification and Approval of New Aviation Turbine
generate cost estimates where data is not currently available Fuels and Fuel Additives[15].
outside of private and proprietary research. Assessing the Jet fuel blendstock produced through the ATJ pathway is
differences between implementations of these routes will assist called ATJ-SPK (synthetic paraffinic kerosene) and is approved
in understanding the engineering and economic challenges and by ASTM D7566 as part of Annex A5. Currently, only ATJ-SPK
provide information to elucidate the role of the ATJ pathway in produced from an ethanol or isobutanol intermediate is allowed
future research and commercial projects. up to a 50% maximum blend. ATJ-SPK derived from other
alcohols or mixed alcohols are not currently allowed, but ASTM
states that they do intend to expand the standard to include
1.2 Overview of ATJ Fuel and Conversion additional alcohols once sufficient test data is available [16,17,18]
Process and Commercial Development (the standard originally only allowed isobutanol, but was revised
in 2018 to include ethanol as well). The specification defines
A number of companies have been developing the ATJ ATJ-SPK as alcohols processed through dehydration,
process toward the goal of commercialization, with some oligomerization, hydrogenation, and fractionation. Any fuel not
variations between them. Leading the efforts in regulatory produced through these steps must seek its own qualification to
approval of ATJ derived fuel are two companies specializing in be used as a jet fuel blendstock, including other catalytic alcohol
advanced biochemically engineered fermentation processes: upgrading processes such as the one developed by Vertimass
Gevo, Inc and LanzaTech. Gevo, which has partnered with and Oak Ridge National Lab[19].
Alaska Airlines for a corn sugar-based ATJ demonstration flight Although many requirements are identical between the
and a cellulosic sugar-based flight as part of the larger D1655 and D7566 fuel specifications, several additional
Northwest Advanced Renewables Alliance (NARA) stipulations are added for alternative fuels; the differences
consortium[11]. Gevo touts a proprietary isobutanol fermentation between them for ATJ-SPK are provided in supplementary
process which utilizes an engineered yeast strain and an document A, Table A1. Numerous concerns regarding specific
advanced integrated separations system called the Gevo differences between synthetic chemical blends and fit-for-
Integrated Fermentation Technology (GIFT) process. LanzaTech purpose petroleum distillates has resulted in stricter
specializes in the fermentation of gas feedstocks, including steel requirements for alternative fuels.
mill flue gas streams and gasified materials. LanzaTech has
recently demonstrated successful production of SAJF from gas-
fermented ethanol in partnership with Virgin Atlantic and Pacific 1.2.2 Production of Alcohols as Jet Fuel
Northwest National Laboratory[12]. Other companies including Intermediates
Butamax and Cobalt Technologies have also contributed to the
development of biorenewable butanol production, although they The general ATJ concept is not specific as to the type of
are no longer pursuing ATJ commercialization[13]. Another alcohol fed to catalytic upgrading to hydrocarbons. Several
approach to ATJ commercialization is the addition of alcohol alcohols currently derived from renewable feedstocks have been
upgrading to conventional ethanol production; Byogy takes this under consideration for use in ATJ conversion including ethanol,
approach primarily aimed to utilize the large sugarcane ethanol n-butanol, and iso-butanol. While yeast fermentation of sugar
industry in Brazil[14]. from edible plants is often claimed as the oldest biochemical
conversion process developed by mankind, the fermentation of
saccharides from non-food plant biomass or other non-
1.2.1 Certification and Qualification of conventional carbon sources requires more sophisticated
Alternative Jet Fuel from ATJ techniques often involving modified microbes and additional
process units. Thermochemical routes to convert biomass to
To deploy a commercial SAJF production operation in the alcohols may alternately be used, often through gasification and
United States, the technology pathway must undergo approval catalytic steps, although pathways using mixed oxygenates
and meet standards set by ASTM International. A thorough other than alcohols are typically explored as well [14e,20].
review of the background of this process is provided by Wilson, The production of alcohols higher than ethanol through
et.al.[15]. The conventional standard for jet fuel is defined by biochemical routes has been thoroughly investigated, and
Conversion Cost ATJ- $0.86 $0.52 Figure 2. Base purchased equipment cost breakdown for standalone ATJ
SPK ($/gal) cases at a scale of 200 ton/day feed.
Purchased Equipment
4.4 2.6 Table 6. Operating Expenses in MM$ / year
Cost (PEC)
Diesel Production
Table 7. Fermentation Unit Parameters 2.26 0 0
Rate, MMgal/yr
Purchased
Equipment Cost 7.7 7.7 15.4
(MM$) Although isobutanol fermentation may theoretically reach
Variable
up to 80% of the maximum yield of ethanol fermentation, actual
Operating 1.2 1.2 2.4 yields achieved in practice may differ depending on the specific
Costs (MM$) fermentation process. Typical modern corn ethanol process can
attain a fermentation yield of 98% theoretical maximum [39].
Isobutanol yield from proprietary processes are not available in
detail, but Gevo announced they achieved 1.80 to 1.85 gallons average cost of ethanol, an isobutanol price of 1.41 times larger
of isobutanol per bushel of corn in 2015 (about 34.4% from ($755/ton) results in equal selling prices through both pathways
sugars, or 83.5% of theoretical maximum for isobutanol) [40]. in our models. In an integrated biorefinery, the price of alcohol
Using these fermentation yield figures (98% and 83.5% will typically represent a function of both the price of feedstock at
theoretical), the above conversion costs become $2.52 for the gate and conversion cost of feedstock to alcohols, both
ethanol and $2.21/$3.37 for the isobutanol cases. adding considerably to the cost. The use of extremely low-cost
feedstocks, such as steel mill flue gas as in some
implementations by LanzaTech, can greatly reduce the final
2.3 Sensitivity Analysis and Effect of Alcohol product selling price.
Price To assess the impact of variations in assumptions and
process performance within the process model, sensitivity
A straightforward way to evaluate the comparative costs of analysis results for both Core ATJ models is shown in Figure 4.
alcohol-to-jet conversion from ethanol and isobutanol is to This analysis demonstrates the effect of an increase or decrease
approach the cost using a total alcohol production price. The in a cost category for each model. Each input is varied to reflect
uncertainty of costs using an alternate or advanced fermentation a range of 50% to 150% of the base case scenario.
process is then contained within this price. This approach
estimates a general trend in the relationship between ATJ
upgrading costs from different alcohol intermediates, although it
should be noted that any realistic scenario involves additional Ethanol Intermediate
variables. A plot of these data is given in Figure 3. The vertical Conversion Cost ($/gal)
dotted line at $534/ton ($1.76/gal) denotes the 2013 to 2017 $0.6 $0.7 $0.8 $0.9 $1.0 $1.1
average cost of ethanol production[41]. At this price for ethanol,
the cost of alcohol feedstock makes up 79.2% of the MSP in the CapEx
ethanol-to-jet base case scenario.
Fixed OpEx
Utilities Costs
MSP
($/gal) Catalyst Price
$10.00
Hydrogen Price
$9.00 Ethanol
$8.00 Base Case: $0.821/gallon
Isobutanol
$7.00
$6.00
$5.00
Isobutanol Intermediate
$4.00
Conversion Cost ($/gal)
$3.00
$0.4 $0.5 $0.6 $0.7
$2.00
$1.00 CapEx
3. Conclusions and Recommendations greater mass yield in terms of alcohol conversion. Although
there are trade-offs between the conversion costs from ethanol
Considering the consistent and rising demand for aviation and isobutanol, the deciding factor between which process
fuels worldwide, the alcohol-to-jet pathway offers a solution for achieves better economics is the cost of producing the alcohol
alcohol producers to enter the market for drop-in fossil fuel intermediate. Since the cost of producing alcohols through
alternatives. New alcohol production capacity using new and fermentation is a function of both the fermentation unit and the
high-tech fermentation technologies to convert industry residuals cost of sugar (or alternative feedstock) price, the selling price of
such as flue gasses or lignocellulosic residues may also see the ATJ fuel is highly dependent on the technology used for alcohol
adoption of ATJ conversion as well in the near future. Several production. An alcohol-production process with a high carbon
companies are achieving varying levels of success in developing yield from a low-cost feedstock is ideal.
the implementation of the ATJ process as a route to improve the It should be noted that public policy-based incentives for
commercial viability of advanced fermentation technologies. biofuels production such as those offered by the Renewable
Recent qualification of ATJ fuel into ASTM standards and its Fuel Standard or the Low Carbon Fuel Standard in the United
demonstration in commercial aircraft also indicates momentum States can significantly affect the decision-making of biofuels
toward further developments and improvements to the process businesses. The ability to generate renewable identification
in the near future. numbers (RINs) or other carbon credits may ultimately
The ATJ pathway enables the use of alcohols from a determine the economics of any SAJF pathway. The ability to
variety of sources to be used as a platform molecule for jet fuel upgrade alcohols as a platform molecule, produced from a
production and no particular alcohol production strategy is variety of sugar, waste, cellulosic, and other sources, may allow
required to generate a qualifying ATJ-SPK fuel as long as it SAJF producers the flexibility to appropriately capitalize on both
produces either ethanol or isobutanol. Both the conventional low cost and incentivized feedstocks that are available.
ethanol industry, such as corn or sugarcane-based fermentation, The models explored in this study represent portions of a
as well as businesses investing in new and advanced alcohol complete biorefinery that would realistically implement ATJ
production technologies can benefit from the ability to enter conversion. The success of ATJ biorefinery projects would rely
drop-in fuel markets using the ATJ pathway. With further on numerous other factors including feedstock availability and
advances in conversion technologies, even lignocellulosic cost, supply chain and infrastructure, and co-product generation.
biorefinery concepts may utilize ATJ through fermentation of The sales of co-products, including additional fuel cuts besides
cellulose hydrolysate or gasified biomass. jet, has a significant effect on minimum selling price particularly
Although a variety of alcohol process streams, including when the co-product is priced considerably higher or lower than
ethanol, higher alcohols, and mixed alcohols, can theoretically the jet fraction; higher-value co-products would be a major
be used as an intermediate for ATJ conversion, the process benefit to an ATJ process. Feedstock cost shows the greatest
differs considerably in terms of engineering and implementation sensitivity toward improving process economics. However, the
of the process depending on the alcohol used. ASTM Standards production of isobutanol or other higher alcohols over or in
recognize their differences and requires a separate qualification addition to ethanol provides significant improvement, provided
process for a given alcohol; ethanol and isobutanol are the only that the combined cost of alcohol production is not significantly
alcohols currently qualified. Any new AJF pathway based on n- impacted. Further research and development into alcohol-
butanol, mixed alcohols/oxygenates, or other intermediates will production processes that utilize low-cost feedstocks and
not only require separate qualification but will involve differently generate higher alcohols is recommended.
engineered catalyst and separation systems. Several areas have been identified as key bottlenecks that
The primary difference in implementation between ethanol- can determine the viability of ATJ production in the near term.
to-jet and isobutanol-to-jet lie in the configuration and catalyst We make the following recommendations and conclusions
selections involved in dehydration and oligomerization to based on results from our models:
produce higher olefins. Once olefins are produced in the At an average alcohol price in our models, the production
appropriate range, the remaining hydrogenation and of alcohol feedstock for ATJ upgrading is estimated to
fractionation steps are similar regardless of process. In both contribute approximately 80% of the production cost for
cases, the main functional challenge in designing an ATJ jet blendstock at the refinery. Improvements to alcohol
reaction scheme is to drive the formation of oligomers to production to generate low-cost alcohols is key to
maximize yield in the appropriate range needed to meet fuel improving viability of ATJ.
specifications. Although fractionation allows for further Use of higher alcohols can provide favorable
refinement of the product to meet specifications, it is important to thermodynamics for lower cost separation and catalytic
increase value by ensuring as much of the product is recovered upgrading stages, with our models showing a 34% cost
as jet fuel or another marketable co-product. reduction in conversion cost for isobutanol over ethanol.
ATJ from short-chain alcohols like ethanol generally A greater production cost for higher alcohols could easily
provides superior flexibility to generate a wide range of fuel negate this benefit however, depending on the state and
products, due to the more varied nature of the oligomerized costs of advanced fermentation technology used to
ethylene streams. Isobutanol oligomerization, however, carries produce the alcohol.
certain advantages in terms of processing costs and has a
Reactor and catalyst design for the oligomerization unit Cost analysis comparisons were conducted using a
should be directed to efficiently generate product-range discounted cash flow model, with financial and operation
fuels with recycle in mind, to minimize equipment costs assumptions summarized in Table 9. These assumptions are
through smaller recycle requirements.
Within the catalytic upgrading process,
capital expenses contribute a significant
impact on economics. Reduction in
equipment and facilities costs, potentially
through integration with existing industrial
facilities and infrastructure, offers the
largest area for reduction in risk for the
installation of an ATJ conversion unit.
based on recommendations and economic analyses by Bann, et.
Current efforts in the development of this technology are
al., and Petter, et. al.,[14c,49]. Further details of these calculations
carried out by private entities with proprietary processes.
can be found in the supplementary spreadsheets for this paper.
Although our models attempt to capture and predict the
performance of these systems, we cannot conclude that either
the ethanol or isobutanol to jet cases will offer superior
Table 9. Summary of Financial and Operation Assumptions for Cash Flow
economics now or in the future. As separate processes, they Models
offer different advantages depending on many factors, and
should be considered on a case-by-case basis. Biochemical Parameter Assumed Value
production of alcohols from cheap, but relatively difficult to
Cost Year 2015
ferment, feedstocks might achieve a lower production cost using
an ethanol intermediate. Alternately, where conventional sugar Process Uptime 90%
feedstocks are available, production of higher alcohols may be a
preferred strategy to reduce cost. Plant financing 30% equity
Inflation 2%
4.1 Process Design Cases and Cost Discount Rate, Real/Nominal 10% / 12.2%
Estimation Working Capital 20% yearly OPEX
Estimates for the capital and operating expenses for Depreciation schedule 7 years, MACRS schedule
various stages of the process were collected from literature
Construction spending schedule (% 8% first year, 60% second year,
when available, augmented by our own process simulations
of FCI) 32% third year
generated using Aspen Plus. Cost estimate data was collected
from Humbird, et. al.[44] for details of ethanol production and Maintenance 6% TPEC
separation (also used to estimate isobutanol production costs)
as well as Tan, et. al.[14e] for data regarding catalytic reactor
costs. Details for the Core ATJ process and isobutanol
separation were gathered using Apsen Plus simulations
described below. Details of the references for capital and
operating cost estimates are available in the spreadsheets 4.2 Process Modelling and Simulation
contained in the supplementary documents of this report. To
estimate total capital costs, a factored approach based from Aspen Plus simulations were used to help estimate
Peters and Timmerhaus[45] was used to correlate additional process information (mass/energy balance, module costs, and
costs such as installation, outside battery-limits, and indirect utility requirements) for the catalytic conversion steps and for
costs from the costs of major process equipment and the isobutanol/water separation. Key differences are present
assumption that the process is an "add-on" to an existing facility between the upgrading process for ethanol and isobutanol,
Variable operating expenses for utilities and materials which were modeled separately. Although the costs for the
were based on process models with cost data from EIA, dehydration of ethanol to ethylene has already been extensively
Humbird et. al., Chu et. al., and Turton et. al., [44,46]. The cost of studied in literature [31,33,50], the process was modeled in our
steam delivery was estimated based on the natural gas costs for simulations to maintain consistent analyses between isobutanol
equivalent energy rates. Fixed operating expenses were and ethanol cases. Figure 6 includes a block diagram of the
adapted from Peters, et. al.,[45] for maintenance, Jones et. al.,[47] process flow units for both Core ATJ units. Detailed diagrams
for taxes and insurance, and Marrs et. al., [48] for cost of labor.
showing the unit operations in each model are provided in the C8 olefins directed to the bottoms product. Distillate is recycled
supplementary documents, Figures A1 and A2. through the oligomerization reactor where olefins further grow
reacting with fresh feed. The presence of a higher amount of
Figure 6. Block Diagram of the ATJ Process Model light olefins results in a larger recycle ratio and the need for a
larger reactor. Catalyst costs and lifetime are based on Tan, et.
al.[9]. A 2% purge is included from the recycle steam.
Process simulations were carried out using the Unifac A 3:1 molar feed of hydrogen is maintained to the
thermodynamic package and components from the Aspen hydrogenation reactor. Due to the excess hydrogen feed, a
databanks as pure compounds for water, ethanol, isobutanol, 100% conversion is assumed and the recycle system is included
ethylene, and isobutylene. Mixtures of olefins and SPK are to reuse hydrogen. The gas recycle system results in hydrogen
simulated using model compounds; higher olefin and paraffin usage close to the theoretical requirement. This includes
mixtures are grouped by carbon numbers in the lengths equipment for gas/liquid separation at 50° C and 200 psig, as
dominantly produced. well as a compressor for recycled gas. A 2% purge stream is
For each reactor system (dehydration, oligomerization, and included to remove impurities and may be used as boiler fuel to
hydrogenation), equipment for the reactors, heat exchangers, recover its energy.
pumps/compressors, and separation units needed for A finishing section was added to make final adjustments in
maintaining recycle are simulated. Costs used for alcohol/water product distribution and properties, completing the process of
separation includes costs due to added capacity to a co-located generating the fuel blendstock. This was modeled as the
unit for fermentation broth separation. The conditions of each addition of two distillation columns, both similar in design to the
reactor (temperature/pressure) were assumed based on column used in the oligomerization loop. The real
literature values and the actual conversion of each is simplified implementation of the process may involve more complex
with fixed single pass conversion parameters and product fractionation of multiple products or removal of a significant
distributions also assumed based on literature. The operating portion of product during finishing, but for the purposes of this
conditions of each reactor may vary between different model it was assumed to have no effect on the ultimate yield or
implementations, depending on specific catalyst performance distribution of the product. Practically, the fuel blendstock
and process streams. A summary of some of these assumed production will include a range of fuels in addition to jet,
key parameters is shown in Table 10 and more detailed potentially including naphtha, gasoline, and diesel although the
descriptions follow.
Dehydration reactors are
assumed to achieve a 90% Table 10. Reactor Conditions Used in Core ATJ Models
single-pass conversion of
[31c,34] [14e,20a,25,30b,35a] [14e,20a,25]
alcohol. The product from Dehydration Oligomerization Hydrogenation
dehydration is separated,
Ethanol Isobutanol Ethanol Isobutanol Ethanol and Isobutanol
removing water and unreacted
alcohols to be sent back to Temperature [°C] 340 325 250 100 100
water/alcohol separation for
recycle[31b,33,34]. Ethylene Pressure [psig] 55 60 300 250 250
separation involves higher 90% 90% 40% C10 20% C8
Single Pass
pressures than isobutene 20% C8, C12 70% C12 100%
Conversion/Distribution 10% C6, C16 10% C16
separation as well as a
requirement for very low recycle integrated with recycle designed to drive 3:1 molar feed of H2;
Recycle Configuration separation of feed conversion to higher olefins (C12+) recycle of H2 is
temperature refrigerant. A
alcohols included
molecular sieve is included to
further eliminate water from the
distillate stream; nearly
complete removal of water is distribution of products varies depending on implementation[14e,f].
necessary to avoid contamination in the oligomerization reactor In these models, production of jet range is favored although
system. some portion of the jet range product is assumed to be
The design of oligomerization reactor systems will differ fractioned off in order to attain a distillation curve necessary to
depending on the selected catalyst. It is not the goal of this meet jet fuel specifications. The remaining hydrocarbon product
model to assess the performance of any individual catalyst or is treated as either a gasoline or diesel co-product. To relate the
design, but to predict and compare the overall costs following sale of these fractions to the selling price of jet fuel, both fuel co-
common design principles and assumptions. A heterogeneous products are correlated linearly to the calculated minimum
catalyst reactor system is modeled with a recycle configuration selling price of jet fuel according to EIA data from 1983 through
to drive the reaction to the target carbon range. A distillation 2016[51].
column separates the reactor product. Light olefins (primarily C8 Detailed cost estimates of an ethanol separation unit is
and smaller) are recovered in the distillate with a target of 10% available in the NREL corn stover ethanol facility report [44], which
was adapted for use in this model. The separation of butanol Tables 11 and 12 provide additional cost estimation details
and isobutanol, however, is carried out using a separate for both Core ATJ models, broken down to the three major
separation scheme. Cost and utility requirements for this process units. Installation costs are estimated as part of the ratio
process was estimated using an Aspen Plus model diagrammed factors outlined by Peters, et al., which are also used to estimate
in Figure 7. outside battery limits costs. Expanded versions of these tables,
with process flow rates and costs/utility usage for individual unit
operations (Tables A2, A3, and A4) are available in the
supplementary documents.
Primary Flow Streams Feed Rate: 308 Feed Rate: 169 Feed Rate: 165
(lb/min) Product: 169 Product: 165 Product: 167
To Recycle: 139
Primary Flow Streams Feed Rate: 308 Feed Rate: 207 Feed Rate: 205
(lb/min) Product: 207 Product: 205 Product: 207
To Recycle: 101
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FULL PAPER
The ATJ Process provides a $10.00 Scott Geleynse, Kristin Brandt, Manuel
promising pathway for the production $9.00 Garcia-Perez, Michael Wolcott, Xiao
of alternative drop-in hydrocarbon $8.00 Zhang
fuels using sustainably produced $7.00
$6.00
alcohols. In this paper, we discuss Page No. – Page No.
$5.00
the key engineering barriers and use $4.00
The Alcohol-to-Jet Conversion
techno-economic assessment to $3.00 Pathway for Drop-In Biofuels:
Ethanol Techno-Economic Evaluation
evaluate potential commercial $2.00
$1.00 Isobutanol
implementations of this imminent
$0.00
alternative fuels process.
$0 $500 $1,000 $1,500
$/gal Alcohol Price ($/ton)